US7052802B2 - Fluorinated carbon active material - Google Patents
Fluorinated carbon active material Download PDFInfo
- Publication number
- US7052802B2 US7052802B2 US10/272,415 US27241502A US7052802B2 US 7052802 B2 US7052802 B2 US 7052802B2 US 27241502 A US27241502 A US 27241502A US 7052802 B2 US7052802 B2 US 7052802B2
- Authority
- US
- United States
- Prior art keywords
- battery
- conductive material
- positive electrode
- carbon
- carbon fluoride
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired - Lifetime, expires
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- QLOAVXSYZAJECW-UHFFFAOYSA-N methane;molecular fluorine Chemical compound C.FF QLOAVXSYZAJECW-UHFFFAOYSA-N 0.000 title abstract description 4
- 239000002388 carbon-based active material Substances 0.000 title 1
- 239000004020 conductor Substances 0.000 claims abstract description 32
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 22
- 239000010931 gold Substances 0.000 claims abstract description 21
- PCHJSUWPFVWCPO-UHFFFAOYSA-N gold Chemical compound [Au] PCHJSUWPFVWCPO-UHFFFAOYSA-N 0.000 claims abstract description 18
- 229910052737 gold Inorganic materials 0.000 claims abstract description 18
- 229910052799 carbon Inorganic materials 0.000 claims abstract description 14
- 229910052751 metal Inorganic materials 0.000 claims abstract description 10
- 239000002184 metal Substances 0.000 claims abstract description 10
- 238000007740 vapor deposition Methods 0.000 claims abstract description 7
- 239000002482 conductive additive Substances 0.000 claims description 14
- TXEYQDLBPFQVAA-UHFFFAOYSA-N tetrafluoromethane Chemical compound FC(F)(F)F TXEYQDLBPFQVAA-UHFFFAOYSA-N 0.000 claims description 14
- 239000011230 binding agent Substances 0.000 claims description 13
- 239000011149 active material Substances 0.000 claims description 8
- 229920001343 polytetrafluoroethylene Polymers 0.000 claims description 7
- 239000004810 polytetrafluoroethylene Substances 0.000 claims description 7
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 claims description 5
- 229910052782 aluminium Inorganic materials 0.000 claims description 5
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 claims description 5
- 239000010949 copper Substances 0.000 claims description 5
- 239000000203 mixture Substances 0.000 claims description 5
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 claims description 5
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims description 4
- 239000002033 PVDF binder Substances 0.000 claims description 4
- 239000004372 Polyvinyl alcohol Substances 0.000 claims description 4
- 229920002451 polyvinyl alcohol Polymers 0.000 claims description 4
- 229920002981 polyvinylidene fluoride Polymers 0.000 claims description 4
- 229920002134 Carboxymethyl cellulose Polymers 0.000 claims description 3
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 claims description 3
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 claims description 3
- 229910052802 copper Inorganic materials 0.000 claims description 3
- 239000003792 electrolyte Substances 0.000 claims description 3
- -1 polytetrafluoroethylene Polymers 0.000 claims description 3
- 239000010948 rhodium Substances 0.000 claims description 3
- 239000010936 titanium Substances 0.000 claims description 3
- BQCADISMDOOEFD-UHFFFAOYSA-N Silver Chemical compound [Ag] BQCADISMDOOEFD-UHFFFAOYSA-N 0.000 claims description 2
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 claims description 2
- 229910052741 iridium Inorganic materials 0.000 claims description 2
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 claims description 2
- 229910052763 palladium Inorganic materials 0.000 claims description 2
- 229910052697 platinum Inorganic materials 0.000 claims description 2
- 229910052703 rhodium Inorganic materials 0.000 claims description 2
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 claims description 2
- 229910052709 silver Inorganic materials 0.000 claims description 2
- 239000004332 silver Substances 0.000 claims description 2
- 229920003048 styrene butadiene rubber Polymers 0.000 claims description 2
- 229910052719 titanium Inorganic materials 0.000 claims description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 claims 1
- VYZAMTAEIAYCRO-UHFFFAOYSA-N Chromium Chemical compound [Cr] VYZAMTAEIAYCRO-UHFFFAOYSA-N 0.000 claims 1
- GYHNNYVSQQEPJS-UHFFFAOYSA-N Gallium Chemical compound [Ga] GYHNNYVSQQEPJS-UHFFFAOYSA-N 0.000 claims 1
- 229910052765 Lutetium Inorganic materials 0.000 claims 1
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 claims 1
- ZOKXTWBITQBERF-UHFFFAOYSA-N Molybdenum Chemical compound [Mo] ZOKXTWBITQBERF-UHFFFAOYSA-N 0.000 claims 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical compound [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 claims 1
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims 1
- ATJFFYVFTNAWJD-UHFFFAOYSA-N Tin Chemical compound [Sn] ATJFFYVFTNAWJD-UHFFFAOYSA-N 0.000 claims 1
- HCHKCACWOHOZIP-UHFFFAOYSA-N Zinc Chemical compound [Zn] HCHKCACWOHOZIP-UHFFFAOYSA-N 0.000 claims 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 claims 1
- 230000003213 activating effect Effects 0.000 claims 1
- 229910052787 antimony Inorganic materials 0.000 claims 1
- WATWJIUSRGPENY-UHFFFAOYSA-N antimony atom Chemical compound [Sb] WATWJIUSRGPENY-UHFFFAOYSA-N 0.000 claims 1
- 229910052788 barium Inorganic materials 0.000 claims 1
- DSAJWYNOEDNPEQ-UHFFFAOYSA-N barium atom Chemical compound [Ba] DSAJWYNOEDNPEQ-UHFFFAOYSA-N 0.000 claims 1
- 229910052790 beryllium Inorganic materials 0.000 claims 1
- ATBAMAFKBVZNFJ-UHFFFAOYSA-N beryllium atom Chemical compound [Be] ATBAMAFKBVZNFJ-UHFFFAOYSA-N 0.000 claims 1
- 229910052793 cadmium Inorganic materials 0.000 claims 1
- BDOSMKKIYDKNTQ-UHFFFAOYSA-N cadmium atom Chemical compound [Cd] BDOSMKKIYDKNTQ-UHFFFAOYSA-N 0.000 claims 1
- 229910052791 calcium Inorganic materials 0.000 claims 1
- 239000011575 calcium Substances 0.000 claims 1
- 229910052804 chromium Inorganic materials 0.000 claims 1
- 239000011651 chromium Substances 0.000 claims 1
- 229910017052 cobalt Inorganic materials 0.000 claims 1
- 239000010941 cobalt Substances 0.000 claims 1
- GUTLYIVDDKVIGB-UHFFFAOYSA-N cobalt atom Chemical compound [Co] GUTLYIVDDKVIGB-UHFFFAOYSA-N 0.000 claims 1
- 229910052733 gallium Inorganic materials 0.000 claims 1
- 229910052735 hafnium Inorganic materials 0.000 claims 1
- VBJZVLUMGGDVMO-UHFFFAOYSA-N hafnium atom Chemical compound [Hf] VBJZVLUMGGDVMO-UHFFFAOYSA-N 0.000 claims 1
- 229910052738 indium Inorganic materials 0.000 claims 1
- APFVFJFRJDLVQX-UHFFFAOYSA-N indium atom Chemical compound [In] APFVFJFRJDLVQX-UHFFFAOYSA-N 0.000 claims 1
- 229910052742 iron Inorganic materials 0.000 claims 1
- OHSVLFRHMCKCQY-UHFFFAOYSA-N lutetium atom Chemical compound [Lu] OHSVLFRHMCKCQY-UHFFFAOYSA-N 0.000 claims 1
- 229910052749 magnesium Inorganic materials 0.000 claims 1
- 239000011777 magnesium Substances 0.000 claims 1
- 229910052750 molybdenum Inorganic materials 0.000 claims 1
- 239000011733 molybdenum Substances 0.000 claims 1
- 229910052759 nickel Inorganic materials 0.000 claims 1
- 229910052758 niobium Inorganic materials 0.000 claims 1
- 239000010955 niobium Substances 0.000 claims 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 claims 1
- 229910052762 osmium Inorganic materials 0.000 claims 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 claims 1
- 229910052699 polonium Inorganic materials 0.000 claims 1
- HZEBHPIOVYHPMT-UHFFFAOYSA-N polonium atom Chemical compound [Po] HZEBHPIOVYHPMT-UHFFFAOYSA-N 0.000 claims 1
- 229910052702 rhenium Inorganic materials 0.000 claims 1
- WUAPFZMCVAUBPE-UHFFFAOYSA-N rhenium atom Chemical compound [Re] WUAPFZMCVAUBPE-UHFFFAOYSA-N 0.000 claims 1
- 229910052707 ruthenium Inorganic materials 0.000 claims 1
- 229910052706 scandium Inorganic materials 0.000 claims 1
- SIXSYDAISGFNSX-UHFFFAOYSA-N scandium atom Chemical compound [Sc] SIXSYDAISGFNSX-UHFFFAOYSA-N 0.000 claims 1
- 229910052710 silicon Inorganic materials 0.000 claims 1
- 239000010703 silicon Substances 0.000 claims 1
- 229910052712 strontium Inorganic materials 0.000 claims 1
- CIOAGBVUUVVLOB-UHFFFAOYSA-N strontium atom Chemical compound [Sr] CIOAGBVUUVVLOB-UHFFFAOYSA-N 0.000 claims 1
- 229910052715 tantalum Inorganic materials 0.000 claims 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 claims 1
- 229910052713 technetium Inorganic materials 0.000 claims 1
- GKLVYJBZJHMRIY-UHFFFAOYSA-N technetium atom Chemical compound [Tc] GKLVYJBZJHMRIY-UHFFFAOYSA-N 0.000 claims 1
- 229910052716 thallium Inorganic materials 0.000 claims 1
- BKVIYDNLLOSFOA-UHFFFAOYSA-N thallium Chemical compound [Tl] BKVIYDNLLOSFOA-UHFFFAOYSA-N 0.000 claims 1
- 229910052718 tin Inorganic materials 0.000 claims 1
- WFKWXMTUELFFGS-UHFFFAOYSA-N tungsten Chemical compound [W] WFKWXMTUELFFGS-UHFFFAOYSA-N 0.000 claims 1
- 229910052721 tungsten Inorganic materials 0.000 claims 1
- 239000010937 tungsten Substances 0.000 claims 1
- 229910052720 vanadium Inorganic materials 0.000 claims 1
- LEONUFNNVUYDNQ-UHFFFAOYSA-N vanadium atom Chemical compound [V] LEONUFNNVUYDNQ-UHFFFAOYSA-N 0.000 claims 1
- 229910052727 yttrium Inorganic materials 0.000 claims 1
- VWQVUPCCIRVNHF-UHFFFAOYSA-N yttrium atom Chemical compound [Y] VWQVUPCCIRVNHF-UHFFFAOYSA-N 0.000 claims 1
- 229910052725 zinc Inorganic materials 0.000 claims 1
- 239000011701 zinc Substances 0.000 claims 1
- 229910052726 zirconium Inorganic materials 0.000 claims 1
- 238000000034 method Methods 0.000 abstract description 15
- 239000000463 material Substances 0.000 abstract description 14
- 229910052744 lithium Inorganic materials 0.000 abstract description 6
- 239000003990 capacitor Substances 0.000 abstract description 5
- 150000002739 metals Chemical class 0.000 abstract description 5
- 238000003860 storage Methods 0.000 abstract description 5
- 239000006229 carbon black Substances 0.000 abstract description 2
- 239000000126 substance Substances 0.000 abstract description 2
- 238000005229 chemical vapour deposition Methods 0.000 abstract 1
- 238000005240 physical vapour deposition Methods 0.000 abstract 1
- 210000004027 cell Anatomy 0.000 description 26
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 description 14
- 238000000151 deposition Methods 0.000 description 13
- 238000000576 coating method Methods 0.000 description 12
- 239000011248 coating agent Substances 0.000 description 10
- 230000008021 deposition Effects 0.000 description 9
- 238000012360 testing method Methods 0.000 description 9
- 229910052786 argon Inorganic materials 0.000 description 7
- 238000004544 sputter deposition Methods 0.000 description 7
- 238000006243 chemical reaction Methods 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 229910001416 lithium ion Inorganic materials 0.000 description 5
- 238000002156 mixing Methods 0.000 description 5
- 239000000843 powder Substances 0.000 description 5
- 239000000758 substrate Substances 0.000 description 5
- WHXSMMKQMYFTQS-UHFFFAOYSA-N Lithium Chemical compound [Li] WHXSMMKQMYFTQS-UHFFFAOYSA-N 0.000 description 4
- 239000006230 acetylene black Substances 0.000 description 4
- 230000009286 beneficial effect Effects 0.000 description 4
- 239000007772 electrode material Substances 0.000 description 4
- 239000010439 graphite Substances 0.000 description 4
- 229910002804 graphite Inorganic materials 0.000 description 4
- 238000009830 intercalation Methods 0.000 description 4
- 229910045601 alloy Inorganic materials 0.000 description 3
- 239000000956 alloy Substances 0.000 description 3
- 230000002687 intercalation Effects 0.000 description 3
- 238000000608 laser ablation Methods 0.000 description 3
- 239000002245 particle Substances 0.000 description 3
- 238000003825 pressing Methods 0.000 description 3
- 210000000352 storage cell Anatomy 0.000 description 3
- 229910001290 LiPF6 Inorganic materials 0.000 description 2
- HBBGRARXTFLTSG-UHFFFAOYSA-N Lithium ion Chemical compound [Li+] HBBGRARXTFLTSG-UHFFFAOYSA-N 0.000 description 2
- 238000003490 calendering Methods 0.000 description 2
- 239000010406 cathode material Substances 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 239000002904 solvent Substances 0.000 description 2
- 229910001220 stainless steel Inorganic materials 0.000 description 2
- 239000010935 stainless steel Substances 0.000 description 2
- BTBUEUYNUDRHOZ-UHFFFAOYSA-N Borate Chemical compound [O-]B([O-])[O-] BTBUEUYNUDRHOZ-UHFFFAOYSA-N 0.000 description 1
- 229920000049 Carbon (fiber) Polymers 0.000 description 1
- 206010011906 Death Diseases 0.000 description 1
- PXGOKWXKJXAPGV-UHFFFAOYSA-N Fluorine Chemical compound FF PXGOKWXKJXAPGV-UHFFFAOYSA-N 0.000 description 1
- 238000004833 X-ray photoelectron spectroscopy Methods 0.000 description 1
- DPXJVFZANSGRMM-UHFFFAOYSA-N acetic acid;2,3,4,5,6-pentahydroxyhexanal;sodium Chemical compound [Na].CC(O)=O.OCC(O)C(O)C(O)C(O)C=O DPXJVFZANSGRMM-UHFFFAOYSA-N 0.000 description 1
- 238000005275 alloying Methods 0.000 description 1
- HSFWRNGVRCDJHI-UHFFFAOYSA-N alpha-acetylene Natural products C#C HSFWRNGVRCDJHI-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
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- 238000005137 deposition process Methods 0.000 description 1
- 238000009826 distribution Methods 0.000 description 1
- 125000002534 ethynyl group Chemical group [H]C#C* 0.000 description 1
- 238000000605 extraction Methods 0.000 description 1
- 229910052731 fluorine Inorganic materials 0.000 description 1
- 239000011737 fluorine Substances 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 238000003780 insertion Methods 0.000 description 1
- 230000037431 insertion Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- VNWKTOKETHGBQD-UHFFFAOYSA-N methane Chemical compound C VNWKTOKETHGBQD-UHFFFAOYSA-N 0.000 description 1
- 239000007773 negative electrode material Substances 0.000 description 1
- 230000001590 oxidative effect Effects 0.000 description 1
- 238000005289 physical deposition Methods 0.000 description 1
- 239000007774 positive electrode material Substances 0.000 description 1
- 238000002360 preparation method Methods 0.000 description 1
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- 239000007787 solid Substances 0.000 description 1
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- 230000000087 stabilizing effect Effects 0.000 description 1
- 238000010301 surface-oxidation reaction Methods 0.000 description 1
- 238000011477 surgical intervention Methods 0.000 description 1
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- H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/10—Energy storage using batteries
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
- Y02E60/13—Energy storage using capacitors
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
- Y10T29/00—Metal working
- Y10T29/49—Method of mechanical manufacture
- Y10T29/49002—Electrical device making
- Y10T29/49108—Electric battery cell making
- Y10T29/49115—Electric battery cell making including coating or impregnating
Definitions
- This invention relates to electrical storage cells, more particularly lithium batteries and capacitors using fluorinated carbon (CFx) as an electrode material.
- the method of the present invention significantly improves overall performance by increasing conductivity through the surface coating by deposition of conductive material.
- Fluorinated carbon (or Carbon Fluoride; hereinafter, CFx) has long been used in a CFx/Li primary battery as a Cathode.
- CFx Fluorinated carbon
- the material has relatively low electrical conductivity requiring a high amount of conductive additive such as carbon to comprise an electrode.
- a CFx electrode contains about 10 wt % of acetylene black (or other conductive additive), reducing a battery's volume energy density significantly.
- the present invention fundamentally involves coating or depositing on the CFx particles a conductive material by means of vapor deposition, such as sputtering, laser ablation, or similar processes. This significantly reduces the amount of conductive additive, improves a CFx cathode's volume energy density, improves CFx's high rate discharge capability, and exhibits more stable electrical characteristics.
- the CFx cathode made by the method of the present invention has deposited on it a conductive material (carbon and/or metal) by means of vapor deposition (e.g., sputtering, or laser ablation), nominally at room temperature, to below 650° C.
- the deposition may take place in a vacuum atmosphere, a low-pressure inert gas atmosphere (e.g., argon) or under pressure to about 10 atmospheres.
- the deposition process uses a carbonaceous organic vapor to deposit carbon and/or metallized carbonaceous organic vapor to deposit metal with or without carbon, or an inert atmosphere (e.g., argon).
- a follow-on heat treatment may also be employed at temperatures up to around 650° C. However, the best mode of the present invention does not require such treatment.
- Vapor deposition in a vacuum or low pressure argon gas results in the CFx being surface coated. Vapor deposition in a pressurized atmosphere (and optionally at elevated temperatures to about 650° C.) forces the conductive material into the CFx particle.
- CFx materials are known in the art, and are commercially available, for example, from Daikin Industries, LTD, Japan.
- Various processes are used to produce CFx, with some being described as “high temperature”, or “HT”, and some being “low temperature”, or “LT”. Examples of each can be found described in U.S. Pat. Nos. 5,712,062 and 6,068,921 to Yamana et al, assigned to Daikin Industries, Ltd., Osaka, Japan, and in U.S. Pat. No. 6,358,649 to Yazami et al., entitled, “Carbons containing fluorine, method of preparation thereof and use as electrode material,” all of which are hereby incorporated herein by reference in their entirety.
- the material of Yazami et al. is reportedly more conductive that other types known in the art, and therefore may be preferred for use in the present invention.
- Preferred deposition materials are gold, silver, platinum, rhodium, palladium, iridium, and carbon which have low contact resistance. Alloys of the most preferred metals are possible, and superior to use of the less-preferred materials. Standard, well-known coating or deposition techniques may be utilized including both chemical and physical deposition, coating, argon sputtering, vacuum sputtering, laser ablation, or similar processes. Low temperature vapor deposition may be utilized in which a carbonaceous gas, such as acetylene, is heated to deposit carbon onto CFx particles.
- a carbonaceous gas such as acetylene
- Metals that have a tendency for high surface oxidation may be coated with lower oxidizing metals.
- copper or aluminum may be deposited, followed by gold to maintain high surface conductivity.
- the conductive layer deposited on the CFx may be metallic or carbon, and can be a porous film or dispersed, discrete island structures.
- “coat” or “coating” shall include all deposition conformations or distributions, whether contiguous or dispersed, regardless of the proportion of surface being covered.
- the inventors have found cells made utilizing gold coated CFx exhibit lower internal resistance, higher overall voltage, and much more stable voltage characteristics. Furthermore, vapor-depositing the conductive material onto CFx requires less conductive material but provides better contact than simply mixing conductive additive power with CFx.
- the same cathode of the present invention may also be advantageously used in secondary cells, capacitors, and in devices combining features of capacitors and electrical storage cells.
- electrolyte salts including LiPF6 or Lithium bis(oxalato)borate (LiBOB).
- FIG. 1 is a graph of discharge voltage profile of a test cell made according to the present invention compared with a reference cell.
- the present invention resulted from the discovery that coating CFx with conductive material, rather than mixing it with such material as carbon, improved its electrical characteristics, including increased conductivity, increased volume energy density, more constant discharge voltages, and higher overall voltage.
- a sandwich type gold coated CFx cell and a reference sandwich type conventional CFx cell were produced in accordance with the invention.
- the test cell cathode material was prepared by argon sputtering deposition of gold on CFx. The deposition was carried out as follows:
- a glass plate with 1.6 g CFx powder was placed in a vacuum chamber.
- the vacuum chamber was evacuated to approximately 50–80 millitorr.
- the vacuum chamber was filled with Ar gas. Pressure was kept at 80 millitorr.
- Plasma current was kept around 15 milliamperes.
- the gold was permitted to deposit on the CFx powder five times for 3 minutes each time. Between each sputtering deposition interval, the powder was agitated.
- the CFx so prepared was then used in assembling the test cell.
- the reference cell was prepared in every respect in the same way, except there was no deposition of gold or other conductive material on the CFx.
- the anode in both cells was pure lithium metal with Cu substrate.
- the electrolyte was a salt consisting of 1.2 molar LiPF6 in 25 wt % EC, 75 wt % DEC and a cathode according to the following composition:
- the above electrode composition is believed by the inventors to constitute the best mode of the present invention.
- the use of argon sputtering is believed to be the best mode for depositing the conductive material (gold) onto the CFx.
- binders may be substituted or added, including polyvinylidene fluoride (PVDF), polyvinyl alcohol (PVA), and styrene butadiene rubber (SBR).
- PVDF polyvinylidene fluoride
- PVA polyvinyl alcohol
- SBR styrene butadiene rubber
- other substrates besides aluminum including but not limited to stainless steel, titanium, and alloys thereof, with aluminum and stainless steel being preferred.
- the conductive additive e.g., acetylene black
- the conductive additive e.g., acetylene black
- the conductive additive e.g., acetylene black
- Other types of carbon black or other conductive materials such as graphite may be substituted for acetylene black, or added to it.
- the amount of binder required is partly dependent on the amount of conductive additive used; because of the large surface area of the conductive additive, if the amount of conductive additive is reduced from 10 wt % to about 5 wt %, the total amount of binder may be reduced from 5 wt % to between 1 and 3 wt %.
- FIG. 1 shows the comparative results of pulse discharge testing of both cells.
- Pulse discharge testing of test cells made according to the present method and reference cells made without deposition of a conductive material on the CFx cathode over approximately 1000 minutes (60,000 seconds) of 0.005 C with a discharge pulse of 0.5 C for 10 ms at every 10 minutes (600 seconds) demonstrated the highly beneficial effects of the present invention.
- the two lower traces 100 and 104 represent the respective voltages measured during each 0.5 C pulse discharge (“pulse discharge voltage”).
- Trace 100 is the pulse discharge voltage of the cell with untreated CFx.
- Trace 104 is the pulse discharge voltage of the cell with gold-coated CFx.
- the upper traces 108 and 112 represent the respective cell voltages during the 10-minute 0.005 C discharge (“normal discharge voltage”).
- Trace 108 is the normal discharge voltage of the cell with untreated CFx.
- Trace 112 is the normal discharge voltage of the cell having a gold-coated CFx cathode. It may be seen that the reference cells (no gold) exhibited about 0.7 V or more drop during each pulse discharge, while the test cells (with gold) dropped only about 0.5 V. Moreover, the reference battery voltage in the reference cell initially dropped from about 3.25 V to about 2.5 V and gradually climbed back to a peak of about 2.6 V over the first 25,000 seconds before it began to drop off gradually to 2.5 V over the course of the pulse discharge.
- the reference cells voltages dropped to 1.7 V to 1.9 V.
- the test cells (with gold deposited on CFx) dropped to a minimum of 2.1 V to 2.2 V. Therefore, cells made according to the present method will operate devices requiring a 2.0 V minimum, as the cells will maintain at least 2.0 volts throughout their useful life.
- the present invention is particularly suited to medical devices, notably implanted batteries where stability, longevity, safety are paramount, and where changing primary batteries requires surgical intervention.
- the CFx of the present invention may also be mixed with other active materials.
- An “active material” is a chemically reactive material at the positive or negative electrode that takes part in the charge and discharge reactions. In a lithium battery positive electrode, it can be any material capable of absorbing lithium ions. Such materials are well-known to those skilled in the art. Mixing of two or more active materials may be used to improve better end-of-life indication. See e.g., U.S. Pat. No. 5,667,916 issued to Ebel et al. disclosing using two mixed cathode materials, each with a discrete voltage characteristic. In the present invention, mixing of a second or additional active material may be done before or after treating the CFx powder with a conductive coating. If treated after mixing, the entire mixture of powders may receive beneficial results.
- the second or more active materials should be in an amount less than that of the CFx, and preferably less than about 20 wt % of the CFx.
- the method of the present invention solves a different problem, that problem being high contact resistance in the positive active material, CF x .
- CF x is a very different material from graphite, and the reaction of Li ion with CF x is not an intercalation reaction. Li ions do not intercalate into CF x ; Li ions simply react with CF x and create LiF.
- the present invention does not assist in lithium ion intercalation, but only reduces the contact resistance of CF x .
- the processes provided by the invention enable production of superior-performing electrochemical storage devices that are characterized by relatively stable voltage over their lifetime, improved internal conductivity (and concomitant reduced internal impedance), and improved volumetric energy density (as compared with prior art).
- the invention thereby provides the ability to produce, among other things, storage cells capable of powering devices requiring 2.0 V minimum operating voltage.
- the devices are particularly suited to medical applications, notably implantable medical devices.
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Abstract
Description
TABLE 1 |
Candidate Elements |
Most Preferred | Ag (6.21)*, Au (4.55), Rh (2.08), Ir (1.96) Pt (.96) |
Pd (.95), C (0.2) | |
Less Preferred | Cu (5.88), Al (3.65), Be (3.08), Ca (2.78), Mg (2.33), |
W (1.89), Mo (1.89), Co (1.72), Zn (1.69), Ni (1.43), | |
Cd (1.38), Ru (1.35), In (1.14), Os (1.1), Fe (1.02), | |
Fe (1.02) Sn (0.91), Cr (0.78), Ta (0.76), Tc (0.7), | |
Nb (0.69), Ga (0.67), TL (0.61), Re (0.54), V (0.5), | |
Pb (0.48), Sr (0.47), Si (0.42), Hf (0.33), Ba (0.26), | |
Zr (0.24), Sb (0.24), Ti (0.23), Po (0.22), Sc (0.21), | |
Y (0.17), Lu (0.13). | |
*Numbers in parentheses are conductivity: 105 (Ωcm)−1 |
CFx (+ Au): | 85 wt % | ||
PTFE: | 3 | ||
CMC | |||
2 wt % | |||
Acetylene Black: | 10 wt %. | ||
Claims (27)
Priority Applications (2)
Application Number | Priority Date | Filing Date | Title |
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US10/272,415 US7052802B2 (en) | 2002-10-15 | 2002-10-15 | Fluorinated carbon active material |
US11/387,622 US7503943B2 (en) | 2002-10-15 | 2006-03-22 | Fluorinated carbon active material |
Applications Claiming Priority (1)
Application Number | Priority Date | Filing Date | Title |
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US10/272,415 US7052802B2 (en) | 2002-10-15 | 2002-10-15 | Fluorinated carbon active material |
Related Child Applications (1)
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US11/387,622 Continuation US7503943B2 (en) | 2002-10-15 | 2006-03-22 | Fluorinated carbon active material |
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Publication Number | Publication Date |
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US20040072075A1 US20040072075A1 (en) | 2004-04-15 |
US7052802B2 true US7052802B2 (en) | 2006-05-30 |
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US10/272,415 Expired - Lifetime US7052802B2 (en) | 2002-10-15 | 2002-10-15 | Fluorinated carbon active material |
US11/387,622 Expired - Lifetime US7503943B2 (en) | 2002-10-15 | 2006-03-22 | Fluorinated carbon active material |
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